Title

Author

Defense Date

2014

Document Type

Dissertation

Degree Name

Doctor of Philosophy

Department

Engineering

First Advisor

Gary Atkinson

Abstract

The importance of gamma-ray spectroscopy – the science of determining the distribution of energy in a gamma field – can rarely be overstated. High performance scintillators for gamma-ray spectroscopy in Nuclear Nonproliferation applications and homeland security require excellent energy resolution to distinguish neighboring element and isotope lines while minimizing the time and exposure to do so. Semiconductor detectors operate by converting incident photons directly into electrical pulses, but often have problems of high costs due to constituent segregation and surface states as is the case for Cadmium Zinc Telluride. The ideal scintillator material for gamma spectrometer will therefore requires high light yield, excellent proportionality between light yield and gamma photon energy, and material uniformity. A scintillator should possess the following properties; it should convert the kinetic energy of the generated charged particles (typically K-shell electrons) into detectable visible light. This conversion should be linear-the light yield should be proportional to deposited energy over as wide a range as possible. For good light collection, the medium should be transparent to the wavelength of its own emission. The decay time of the induced luminescence should be short so that fast signal pulses can be generated. The medium should be of good optical quality and subject to manufacture in sizes large enough to be of interest as a practical detector. Its index of refraction should be near that of glass (~1.5) to permit efficient coupling of scintillation light to a photomultiplier tube or other photo-sensor. In the past decade, inorganic scintillator research has focused less on improving the characteristics of known scintillators, but rather on the search for new hosts capable of fast response and high energy resolution. Extensive searches have been made for hosts doped with lanthanide activators utilizing the allowed 5d-4f transition. These 5d-4f transitions are dipole-allowed and thus are about 106 times stronger than the more frequently observed 4f-4f transition in the trivalent rare earth ions. Ce3+, Nd3+ and Pr3+ have been investigated for fast response applications while Ce3+, Eu2+ and Yb2+ stand out as the most promising activators offering high light yield, and high energy resolution. Using a modified Bridgman growth technique we have grown crystals with a low energy resolution of 2.6% at 662 keV, which is lower than the previous 2.8% reported for SrI2:Eu2+. The modified technique (called so for its vertical crystal growth orientation) is necessary due to the anisotropic thermal expansion coefficient of Strontium Iodide. The problem plaguing the growth of the crystal is spontaneous cracking, which usually appear during cooling in the bulk. With the use of a zone separating shield, one can achieve more control of the temperature gradient between the two zones without compromising the actual temperature of the two zones. Additionally the use of codopants, in particular divalent magnesium improved the crystalline quality by acting as a gathering for iodine ions, which led to reduction of defect density.